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1.
Nature ; 631(8019): 98-105, 2024 Jul.
Artigo em Inglês | MEDLINE | ID: mdl-38867037

RESUMO

A key challenge in aerosol pollution studies and climate change assessment is to understand how atmospheric aerosol particles are initially formed1,2. Although new particle formation (NPF) mechanisms have been described at specific sites3-6, in most regions, such mechanisms remain uncertain to a large extent because of the limited ability of atmospheric models to simulate critical NPF processes1,7. Here we synthesize molecular-level experiments to develop comprehensive representations of 11 NPF mechanisms and the complex chemical transformation of precursor gases in a fully coupled global climate model. Combined simulations and observations show that the dominant NPF mechanisms are distinct worldwide and vary with region and altitude. Previously neglected or underrepresented mechanisms involving organics, amines, iodine oxoacids and HNO3 probably dominate NPF in most regions with high concentrations of aerosols or large aerosol radiative forcing; such regions include oceanic and human-polluted continental boundary layers, as well as the upper troposphere over rainforests and Asian monsoon regions. These underrepresented mechanisms also play notable roles in other areas, such as the upper troposphere of the Pacific and Atlantic oceans. Accordingly, NPF accounts for different fractions (10-80%) of the nuclei on which cloud forms at 0.5% supersaturation over various regions in the lower troposphere. The comprehensive simulation of global NPF mechanisms can help improve estimation and source attribution of the climate effects of aerosols.

2.
Proc Natl Acad Sci U S A ; 119(44): e2207329119, 2022 11.
Artigo em Inglês | MEDLINE | ID: mdl-36252100

RESUMO

Increased wildfire events constitute a significant threat to life and property in the United States. Wildfire impact on severe storms and weather hazards is another pathway that threatens society, and our understanding of which is very limited. Here, we use unique modeling developments to explore the effects of wildfires in the western US (mainly California and Oregon) on precipitation and hail in the central US. We find that the western US wildfires notably increase the occurrences of heavy precipitation rates by 38% and significant severe hail (≥2 in.) by 34% in the central United States. Both heat and aerosols from wildfires play an important role. By enhancing surface high pressure and increasing westerly and southwesterly winds, wildfires in the western United States produce (1) stronger moisture and aerosol transport to the central United States and (2) larger wind shear and storm-relative helicity in the central United States. Both the meteorological environment more conducive to severe convective storms and increased aerosols contribute to the enhancements of heavy precipitation rates and large hail. Moreover, the local wildfires in the central US also enhance the severity of storms, but their impact is notably smaller than the impact of remote wildfires in California and Oregon because of the lessened severity of the local wildfires. As wildfires are projected to be more frequent and severe in a warmer climate, the influence of wildfires on severe weather in downwind regions may become increasingly important.


Assuntos
Incêndios Florestais , Aerossóis , Oregon , Estados Unidos , Tempo (Meteorologia) , Vento
3.
Anal Chem ; 96(23): 9524-9534, 2024 Jun 11.
Artigo em Inglês | MEDLINE | ID: mdl-38815054

RESUMO

Quantitative assessment of gas-particle partitioning of individual components within complex atmospheric organic aerosol (OA) mixtures is critical for predicting and comprehending the formation and evolution of OA particles in the atmosphere. This investigation leverages previously documented data obtained through a temperature-programmed desorption-direct analysis in real-time, high-resolution mass spectrometry (TPD-DART-HRMS) platform. This methodology facilitates the bottom-up construction of volatility basis set (VBS) distributions for constituents found in three biogenic secondary organic aerosol (SOA) mixtures produced through the ozonolysis of α-pinene, limonene, and ocimene. The apparent enthalpies (ΔH*, kJ mol-1) and saturation mass concentrations (CT*, µg·m-3) of individual SOA components, determined as a function of temperature (T, K), facilitated an assessment of changes in VBS distributions and gas-particle partitioning with respect to T and atmospheric total organic mass loadings (tOM, µg·m-3). The VBS distributions reveal distinct differences in volatilities among monomers, dimers, and trimers, categorized into separate volatility bins. At the ambient temperature of T = 298 K, only monomers efficiently partition between gas and particle phases across a broad range of atmospherically relevant tOM values of 1-100 µg·m-3. Partitioning of dimers and trimers becomes notable only at T > 360 K and T > 420 K, respectively. The viscosity of SOA mixtures is assessed using a bottom-up calculation approach, incorporating the input of elemental formulas, ΔH*, CT*, and particle-phase mass fractions of the SOA components. Through this approach, we are able to accurately estimate the variations in SOA viscosity that result from the evaporation of its components. These variations are, in turn, influenced by atmospherically relevant changes in tOM and T. Comparison of the calculated SOA viscosity and diffusivity values with literature reported experimental results shows close agreement, thereby validating the employed calculation approach. These findings underscore the significant potential for TPD-DART-HRMS measurements in enabling the untargeted analysis of organic molecules within OA mixtures. This approach facilitates quantitative assessment of their gas-particle partitioning and allows for the estimation of their viscosity and condensed-phase diffusion, thereby contributing valuable insights to atmospheric models.

4.
Environ Sci Technol ; 58(8): 3776-3786, 2024 Feb 27.
Artigo em Inglês | MEDLINE | ID: mdl-38346331

RESUMO

Phenols emitted from biomass burning contribute significantly to secondary organic aerosol (SOA) formation through the partitioning of semivolatile products formed from gas-phase chemistry and multiphase chemistry in aerosol liquid water and clouds. The aqueous-phase SOA (aqSOA) formed via hydroxyl radical (•OH), singlet molecular oxygen (1O2*), and triplet excited states of organic compounds (3C*), which oxidize dissolved phenols in the aqueous phase, might play a significant role in the evolution of organic aerosol (OA). However, a quantitative and predictive understanding of aqSOA has been challenging. Here, we develop a stand-alone box model to investigate the formation of SOA from gas-phase •OH chemistry and aqSOA formed by the dissolution of phenols followed by their aqueous-phase reactions with •OH, 1O2*, and 3C* in cloud droplets and aerosol liquid water. We investigate four phenolic compounds, i.e., phenol, guaiacol, syringol, and guaiacyl acetone (GA), which represent some of the key potential sources of aqSOA from biomass burning in clouds. For the same initial precursor organic gas that dissolves in aerosol/cloud liquid water and subsequently reacts with aqueous phase oxidants, we predict that the aqSOA formation potential (defined as aqSOA formed per unit dissolved organic gas concentration) of these phenols is higher than that of isoprene-epoxydiol (IEPOX), a well-known aqSOA precursor. Cloud droplets can dissolve a broader range of soluble phenols compared to aqueous aerosols, since the liquid water contents of aerosols are orders of magnitude smaller than cloud droplets. Our simulations suggest that highly soluble and reactive multifunctional phenols like GA would predominantly undergo cloud chemistry within cloud layers, while gas-phase chemistry is likely to be more important for less soluble phenols. But in the absence of clouds, the condensation of low-volatility products from gas-phase oxidation followed by their reversible partitioning to organic aerosols dominates SOA formation, while the SOA formed through aqueous aerosol chemistry increases with relative humidity (RH), approaching 40% of the sum of gas and aqueous aerosol chemistry at 95% RH for GA. Our model developments of biomass-burning phenols and their aqueous chemistry can be readily implemented in regional and global atmospheric chemistry models to investigate the aqueous aerosol and cloud chemistry of biomass-burning organic gases in the atmosphere.


Assuntos
Compostos Orgânicos , Fenóis , Biomassa , Aerossóis , Água/química
5.
Environ Sci Technol ; 58(23): 10060-10071, 2024 Jun 11.
Artigo em Inglês | MEDLINE | ID: mdl-38709895

RESUMO

Atmospheric particles play critical roles in climate. However, significant knowledge gaps remain regarding the vertically resolved organic molecular-level composition of atmospheric particles due to aloft sampling challenges. To address this, we use a tethered balloon system at the Southern Great Plains Observatory and high-resolution mass spectrometry to, respectively, collect and characterize organic molecular formulas (MF) in the ground level and aloft (up to 750 m) samples. We show that organic MF uniquely detected aloft were dominated by organonitrates (139 MF; 54% of all uniquely detected aloft MF). Organonitrates that were uniquely detected aloft featured elevated O/C ratios (0.73 ± 0.23) compared to aloft organonitrates that were commonly observed at the ground level (0.63 ± 0.22). Unique aloft organic molecular composition was positively associated with increased cloud coverage, increased aloft relative humidity (∼40% increase compared to ground level), and decreased vertical wind variance. Furthermore, 29% of extremely low volatility organic compounds in the aloft sample were truly unique to the aloft sample compared to the ground level, emphasizing potential oligomer formation at higher altitudes. Overall, this study highlights the importance of considering vertically resolved organic molecular composition (particularly for organonitrates) and hypothesizes that aqueous phase transformations and vertical wind variance may be key variables affecting the molecular composition of aloft organic aerosol.


Assuntos
Espectrometria de Massas , Monitoramento Ambiental , Atmosfera/química , Aerossóis , Poluentes Atmosféricos/análise
6.
Acta Radiol ; 64(8): 2455-2469, 2023 Aug.
Artigo em Inglês | MEDLINE | ID: mdl-37143263

RESUMO

The cerebral arterial system shows a wide spectrum of variations. Minor degrees of anatomic differences can be seen in almost all patients. Recognition of these anatomic variants is essential for the following: evaluating collateral circulation; some anatomic variants may mimic pathology; increased risk for aneurysm formation with some variants (e.g. fenestration, persistent trigeminal artery); dealing with pathologies that can arise with these variations; and for preoperative planning. The anterior and posterior groups of intracranial circulation show numerous anastomoses that play a major role in maintaining adequate blood supply to the cerebral parenchyma. This review focuses on the imaging features of these variants as seen on computed tomography and magnetic resonance imaging with relevant digital subtraction angiography imaging. We also present some case illustrations where understanding of these variants contributed to providing appropriate management.


Assuntos
Artéria Carótida Interna , Aneurisma Intracraniano , Humanos , Angiografia Cerebral , Imageamento por Ressonância Magnética , Artérias Cerebrais , Circulação Cerebrovascular , Aneurisma Intracraniano/diagnóstico por imagem
7.
Proc Natl Acad Sci U S A ; 117(41): 25344-25351, 2020 10 13.
Artigo em Inglês | MEDLINE | ID: mdl-32989149

RESUMO

The large concentrations of ultrafine particles consistently observed at high altitudes over the tropics represent one of the world's largest aerosol reservoirs, which may be providing a globally important source of cloud condensation nuclei. However, the sources and chemical processes contributing to the formation of these particles remain unclear. Here we investigate new particle formation (NPF) mechanisms in the Amazon free troposphere by integrating insights from laboratory measurements, chemical transport modeling, and field measurements. To account for organic NPF, we develop a comprehensive model representation of the temperature-dependent formation chemistry and thermodynamics of extremely low volatility organic compounds as well as their roles in NPF processes. We find that pure-organic NPF driven by natural biogenic emissions dominates in the uppermost troposphere above 13 km and accounts for 65 to 83% of the column total NPF rate under relatively pristine conditions, while ternary NPF involving organics and sulfuric acid dominates between 8 and 13 km. The large organic NPF rates at high altitudes mainly result from decreased volatility of organics and increased NPF efficiency at low temperatures, somewhat counterbalanced by a reduced chemical formation rate of extremely low volatility organic compounds. These findings imply a key role of naturally occurring organic NPF in high-altitude preindustrial environments and will help better quantify anthropogenic aerosol forcing from preindustrial times to the present day.

8.
Environ Sci Technol ; 55(8): 4357-4367, 2021 04 20.
Artigo em Inglês | MEDLINE | ID: mdl-33705653

RESUMO

A major challenge in assessing the impact of aerosols on climate change is to understand how human activities change aerosol loading and properties relative to the pristine/preindustrial baseline. Here, we combine chemical transport simulations and field measurements to investigate the effect of anthropogenic pollution from an isolated metropolis on the particle number concentration over the preindustrial-like Amazon rainforest through various new-particle formation (NPF) mechanisms and primary particle emissions. To represent organic-mediated NPF, we employ a state-of-the-art model that systematically simulates the formation chemistry and thermodynamics of extremely low volatility organic compounds, as well as their roles in NPF processes, and further update the model to improve organic NPF simulations under human-influenced conditions. Results show that urban pollution from the metropolis increases the particle number concentration by a factor of 5-25 over the downwind region (within 200 km from the city center) compared to background conditions. Our model indicates that NPF contributes over 70% of the total particle number in the downwind region except immediately adjacent to the sources. Among different NPF mechanisms, the ternary NPF involving organics and sulfuric acid overwhelmingly dominates. The improved understanding of particle formation mechanisms will help better quantify anthropogenic aerosol forcing from preindustrial times to the present day.


Assuntos
Poluentes Atmosféricos , Aerossóis/análise , Poluentes Atmosféricos/análise , Cidades , Poluição Ambiental , Humanos , Floresta Úmida
9.
Environ Sci Technol ; 55(23): 15680-15693, 2021 12 07.
Artigo em Inglês | MEDLINE | ID: mdl-34775752

RESUMO

Molecular analyses help to investigate the key precursors and chemical processes of secondary organic aerosol (SOA) formation. We obtained the sources and molecular compositions of organic aerosol in PM2.5 in winter in Beijing by online and offline mass spectrometer measurements. Photochemical and aqueous processing were both involved in producing SOA during the haze events. Aromatics, isoprene, long-chain alkanes or alkenes, and carbonyls such as glyoxal and methylglyoxal were all important precursors. The enhanced SOA formation during the severe haze event was predominantly contributed by aqueous processing that was promoted by elevated amounts of aerosol water for which multifunctional organic nitrates contributed the most followed by organic compounds having four oxygen atoms in their formulae. The latter included dicarboxylic acids and various oxidation products from isoprene and aromatics as well as products or oligomers from methylglyoxal aqueous uptake. Nitrated phenols, organosulfates, and methanesulfonic acid were also important SOA products but their contributions to the elevated SOA mass during the severe haze event were minor. Our results highlight the importance of reducing nitrogen oxides and nitrate for future SOA control. Additionally, the formation of highly oxygenated long-chain molecules with a low degree of unsaturation in polluted urban environments requires further research.


Assuntos
Poluentes Atmosféricos , Aerossóis/análise , Poluentes Atmosféricos/análise , Nitratos , Óxidos de Nitrogênio , Compostos Orgânicos/análise
10.
Environ Sci Technol ; 54(7): 3861-3870, 2020 04 07.
Artigo em Inglês | MEDLINE | ID: mdl-32154714

RESUMO

Secondary organic aerosol (SOA) accounts for a large fraction of the tropospheric particulate matter. Although SOA production rates and mechanisms have been extensively investigated, loss pathways remain uncertain. Most large-scale chemistry and transport models account for mechanical deposition of SOA but not chemical losses such as photolysis. There is also a paucity of laboratory measurements of SOA photolysis, which limits how well photolytic losses can be modeled. Here, we show, through a combined experimental and modeling approach, that photolytic loss of SOA mass significantly alters SOA budget predictions. Using environmental chamber experiments at variable relative humidity between 0 and 60%, we find that SOA produced from several biogenic volatile organic compounds undergoes photolysis-induced mass loss at rates between 0 and 2.2 ± 0.4% of nitrogen dioxide (NO2) photolysis, equivalent to average atmospheric lifetimes as short as 10 h. We incorporate our photolysis rates into a regional chemical transport model to test the sensitivity of predicted SOA mass concentrations to photolytic losses. The addition of photolysis causes a ∼50% reduction in biogenic SOA loadings over the Amazon, indicating that photolysis exerts a substantial control over the atmospheric SOA lifetime, with a likely dependence upon the SOA molecular composition and thus production mechanisms.


Assuntos
Poluentes Atmosféricos , Compostos Orgânicos Voláteis , Aerossóis , Modelos Químicos , Material Particulado , Fotólise
11.
Proc Natl Acad Sci U S A ; 114(6): 1246-1251, 2017 02 07.
Artigo em Inglês | MEDLINE | ID: mdl-28115713

RESUMO

Polycyclic aromatic hydrocarbons (PAHs) have toxic impacts on humans and ecosystems. One of the most carcinogenic PAHs, benzo(a)pyrene (BaP), is efficiently bound to and transported with atmospheric particles. Laboratory measurements show that particle-bound BaP degrades in a few hours by heterogeneous reaction with ozone, yet field observations indicate BaP persists much longer in the atmosphere, and some previous chemical transport modeling studies have ignored heterogeneous oxidation of BaP to bring model predictions into better agreement with field observations. We attribute this unexplained discrepancy to the shielding of BaP from oxidation by coatings of viscous organic aerosol (OA). Accounting for this OA viscosity-dependent shielding, which varies with temperature and humidity, in a global climate/chemistry model brings model predictions into much better agreement with BaP measurements, and demonstrates stronger long-range transport, greater deposition fluxes, and substantially elevated lung cancer risk from PAHs. Model results indicate that the OA coating is more effective in shielding BaP in the middle/high latitudes compared with the tropics because of differences in OA properties (semisolid when cool/dry vs. liquid-like when warm/humid). Faster chemical degradation of BaP in the tropics leads to higher concentrations of BaP oxidation products over the tropics compared with higher latitudes. This study has profound implications demonstrating that OA strongly modulates the atmospheric persistence of PAHs and their cancer risks.


Assuntos
Atmosfera/química , Benzo(a)pireno/química , Carcinógenos/química , Neoplasias Pulmonares/induzido quimicamente , Modelos Químicos , Aerossóis , Benzo(a)pireno/efeitos adversos , Clima , Humanos , Oxirredução , Medição de Risco
12.
Environ Sci Technol ; 52(16): 9225-9234, 2018 08 21.
Artigo em Inglês | MEDLINE | ID: mdl-30028598

RESUMO

We developed a parametrizable box model to empirically derive the yields of semivolatile products from VOC oxidation using chamber measurements, while explicitly accounting for the multigenerational chemical aging processes (such as the gas-phase fragmentation and functionalization and aerosol-phase oligomerization and photolysis) under different NO x levels and the loss of particles and gases to chamber walls. Using the oxidation of isoprene as an example, we showed that the assumptions regarding the NO x-sensitive, multigenerational aging processes of VOC oxidation products have large impacts on the parametrized product yields and SOA formation. We derived sets of semivolatile product yields from isoprene oxidation under different NO x levels. However, we stress that these product yields must be used in conjunction with the corresponding multigenerational aging schemes in chemical transport models. As more mechanistic insights regarding SOA formation from VOC oxidation emerge, our box model can be expanded to include more explicit chemical aging processes and help ultimately bridge the gap between the process-based understanding of SOA formation from VOC oxidation and the bulk-yield parametrizations used in chemical transport models.


Assuntos
Gases , Hemiterpenos , Aerossóis , Butadienos , Oxirredução , Pentanos
13.
Faraday Discuss ; 200: 143-164, 2017 08 24.
Artigo em Inglês | MEDLINE | ID: mdl-28581016

RESUMO

When secondary organic aerosol (SOA) particles are formed by ozonolysis in the presence of gas-phase polycyclic aromatic hydrocarbons (PAHs), their formation and properties are significantly different from SOA particles formed without PAHs. For all SOA precursors and all PAHs, discussed in this study, the presence of the gas-phase PAHs during SOA formation significantly affects particle mass loadings, composition, growth, evaporation kinetics, and viscosity. SOA particles formed in the presence of PAHs have, as part of their compositions, trapped unreacted PAHs and products of heterogeneous reactions between PAHs and ozone. Compared to 'pure' SOA particles, these particles exhibit slower evaporation kinetics, have higher fractions of non-volatile components, like oligomers, and higher viscosities, assuring their longer atmospheric lifetimes. In turn, the increased viscosity and decreased volatility provide a shield that protects PAHs from chemical degradation and evaporation, allowing for the long-range transport of these toxic pollutants. The magnitude of the effect of PAHs on SOA formation is surprisingly large. The presence of PAHs during SOA formation increases mass loadings by factors of two to five, and particle number concentrations, in some cases, by more than a factor of 100. Increases in SOA mass, particle number concentrations, and lifetime have important implications to many atmospheric processes related to climate, weather, visibility, and human health, all of which relate to the interactions between biogenic SOA and anthropogenic PAHs. The synergistic relationship between SOA and PAHs presented here are clearly complex and call for future research to elucidate further the underlying processes and their exact atmospheric implications.


Assuntos
Hidrocarbonetos Policíclicos Aromáticos/química , Aerossóis/síntese química , Aerossóis/química , Aerossóis/metabolismo , Gases/química , Estrutura Molecular , Tamanho da Partícula
14.
Environ Sci Technol ; 49(1): 243-9, 2015 Jan 06.
Artigo em Inglês | MEDLINE | ID: mdl-25494490

RESUMO

Secondary organic aerosols (SOA) dominate atmospheric organic aerosols that affect climate, air quality, and health. Recent studies indicate that, contrary to previously held assumptions, at low relative humidity (RH) these particles are semisolid and evaporate orders of magnitude slower than expected. Elevated relative humidity has the potential to affect significantly formation, properties, and atmospheric evolution of SOA particles. Here we present a study of the effect of RH on the room-temperature evaporation kinetics of SOA particles formed by ozonolysis of α-pinene and limonene. Experiments were carried out on α-pinene SOA particles generated, evaporated, and aged at <5%, 50 and 90% RH, and on limonene SOA particles at <5% and 90% RH. We find that in all cases evaporation begins with a relatively fast phase, during which 30-70% of the particle mass evaporates in 2 h, followed by a much slower evaporation rate. Evaporation kinetics at <5% and 50% RH are nearly the same, while at 90% RH a slightly larger fraction evaporates. In all cases, aging the particles prior to inducing evaporation reduces the evaporative losses; with aging at elevated RH leading to a more significant effect. In all cases, the observed SOA evaporation is nearly size-independent.


Assuntos
Aerossóis/química , Cicloexenos/química , Monoterpenos/química , Terpenos/química , Poluentes Atmosféricos/química , Monoterpenos Bicíclicos , Umidade , Cinética , Laboratórios , Limoneno , Volatilização
15.
Proc Natl Acad Sci U S A ; 108(6): 2190-5, 2011 Feb 08.
Artigo em Inglês | MEDLINE | ID: mdl-21262848

RESUMO

Field measurements of secondary organic aerosol (SOA) find significantly higher mass loads than predicted by models, sparking intense effort focused on finding additional SOA sources but leaving the fundamental assumptions used by models unchallenged. Current air-quality models use absorptive partitioning theory assuming SOA particles are liquid droplets, forming instantaneous reversible equilibrium with gas phase. Further, they ignore the effects of adsorption of spectator organic species during SOA formation on SOA properties and fate. Using accurate and highly sensitive experimental approach for studying evaporation kinetics of size-selected single SOA particles, we characterized room-temperature evaporation kinetics of laboratory-generated α-pinene SOA and ambient atmospheric SOA. We found that even when gas phase organics are removed, it takes ∼24 h for pure α-pinene SOA particles to evaporate 75% of their mass, which is in sharp contrast to the ∼10 min time scale predicted by current kinetic models. Adsorption of "spectator" organic vapors during SOA formation, and aging of these coated SOA particles, dramatically reduced the evaporation rate, and in some cases nearly stopped it. Ambient SOA was found to exhibit evaporation behavior very similar to that of laboratory-generated coated and aged SOA. For all cases studied in this work, SOA evaporation behavior is nearly size-independent and does not follow the evaporation kinetics of liquid droplets, in sharp contrast with model assumptions. The findings about SOA phase, evaporation rates, and the importance of spectator gases and aging all indicate that there is need to reformulate the way SOA formation and evaporation are treated by models.


Assuntos
Modelos Químicos , Monoterpenos/química , Transição de Fase , Aerossóis , Monoterpenos Bicíclicos , Temperatura Alta , Cinética , Monoterpenos/síntese química
16.
J Air Waste Manag Assoc ; 64(6): 690-703, 2014 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-25039203

RESUMO

UNLABELLED: Low-density polyethylene (LDPE) plastic is used to keep piled debris from silvicultural activities--activities associated with development and care of forests--dry to enable efficient disposal by burning. The effects of inclusion of LDPE in this manner on smoke emissions are not well known. In a combustion laboratory experiment, 2-kg mixtures of LDPE and manzanita (Arctostaphylos sp.) wood containing 0, 0.25, and 2.5% LDPE by mass were burned. Gaseous and particulate emissions were sampled in real time during the entire flaming, mixed combustion phase--when the flaming and smoldering phases are present at the same time--and during a portion of the smoldering phase. Analysis of variance was used to test significance of modified combustion efficiency (MCE)--the ratio of concentrations of fire-integrated excess CO2 to CO2 plus CO--and LDPE content on measured individual compounds. MCE ranged between 0.983 and 0.993, indicating that combustion was primarily flaming; MCE was seldom significant as a covariate. Of the 195 compounds identified in the smoke emissions, only the emission factor (EF) of 3M-octane showed an increase with increasing LDPE content. Inclusion of LDPE had an effect on EFs of pyrene and fluoranthene, but no statistical evidence of a linear trend was found. Particulate emission factors showed a marginally significant linear relationship with MCE (0.05 < P-value < 0.10). Based on the results of the current and previous studies and literature reviews, the inclusion of small mass proportions of LDPE in piled silvicultural debris does not appear to change the emissions produced when low-moisture-content wood is burned. In general, combustion of wet piles results in lower MCEs and consequently higher levels of emissions. IMPLICATIONS: Current air quality regulations permit the use of burning to dispose of silvicultural piles; however, inclusion of low-density polyethyelene (LDPE) plastic in silvicultural piles can result in a designation of the pile as waste. Waste burning is not permitted in many areas, and there is also concern that inclusion of LDPE leads to toxic air emissions.


Assuntos
Poluentes Atmosféricos/análise , Poluentes Atmosféricos/química , Monóxido de Carbono/análise , Incineração , Polietileno/química , Fumaça/análise , Resíduos , Análise de Variância , Arctostaphylos , Monitoramento Ambiental/métodos , Incêndios , Modelos Químicos , Estados Unidos , Instalações de Eliminação de Resíduos , Madeira
17.
Nat Commun ; 15(1): 4465, 2024 May 25.
Artigo em Inglês | MEDLINE | ID: mdl-38796477

RESUMO

High concentrations of organic aerosol (OA) occur in Asian countries, leading to great health burdens. Clean air actions have resulted in significant emission reductions of air pollutants in China. However, long-term nation-wide trends in OA and their causes remain unknown. Here, we present both observational and model evidence demonstrating widespread decreases with a greater reduction in primary OA than in secondary OA (SOA) in China during the period of 2013 to 2020. Most of the decline is attributed to reduced residential fuel burning while the interannual variability in SOA may have been driven by meteorological variations. We find contrasting effects of reducing NOx and SO2 on SOA production which may have led to slight overall increases in SOA. Our findings highlight the importance of clean energy replacements in multiple sectors on achieving air-quality targets because of high OA precursor emissions and fluctuating chemical and meteorological conditions.

18.
Environ Sci Technol ; 46(22): 12459-66, 2012 Nov 20.
Artigo em Inglês | MEDLINE | ID: mdl-23098132

RESUMO

Polycyclic aromatic hydrocarbons (PAHs), known for their harmful health effects, undergo long-range transport (LRT) when adsorbed on and/or absorbed in atmospheric particles. The association between atmospheric particles, PAHs, and their LRT has been the subject of many studies yet remains poorly understood. Current models assume PAHs instantaneously attain reversible gas-particle equilibrium. In this paradigm, as gas-phase PAH concentrations are depleted due to oxidation and dilution during LRT, particle-bound PAHs rapidly evaporate to re-establish equilibrium leading to severe underpredictions of LRT potential of particle-bound PAHs. Here we present a new, experimentally based picture in which PAHs trapped inside highly viscous semisolid secondary organic aerosol (SOA) particles, during particle formation, are prevented from evaporation and shielded from oxidation. In contrast, surface-adsorbed PAHs rapidly evaporate leaving no trace. We find synergetic effects between hydrophobic organics and SOA - the presence of hydrophobic organics inside SOA particles drastically slows SOA evaporation to the point that it can almost be ignored, and the highly viscous SOA prevents PAH evaporation ensuring efficient LRT. The data show the assumptions of instantaneous reversible gas-particle equilibrium for PAHs and SOA are fundamentally flawed, providing an explanation for the persistent discrepancy between observed and predicted particle-bound PAHs.


Assuntos
Aerossóis/química , Poluentes Atmosféricos/química , Hidrocarbonetos Policíclicos Aromáticos/química , Adsorção , Gases/química , Espectrometria de Massas , Modelos Químicos , Oxirredução , Volatilização
19.
Ambio ; 41 Suppl 1: 68-77, 2012.
Artigo em Inglês | MEDLINE | ID: mdl-22314857

RESUMO

At the international level, India is emerging as a key actor in climate negotiations, while at the national and sub-national levels, the climate policy landscape is becoming more active and more ambitious. It is essential to unravel this complex landscape if we are to understand why policy looks the way it does, and the extent to which India might contribute to a future international framework for tackling climate change as well as how international parties might cooperate with and support India's domestic efforts. Drawing on both primary and secondary data, this paper analyzes the material and ideational drivers that are most strongly influencing policy choices at different levels, from international negotiations down to individual states. We argue that at each level of decision making in India, climate policy is embedded in wider policy concerns. In the international realm, it is being woven into broader foreign policy strategy, while domestically, it is being shaped to serve national and sub-national development interests. While our analysis highlights some common drivers at all levels, it also finds that their influences over policy are not uniform across the different arenas, and in some cases, they work in different ways at different levels of policy. We also indicate what this may mean for the likely acceptability within India of various climate policies being pushed at the international level.


Assuntos
Mudança Climática , Política Ambiental , Governo Federal , Índia , Cooperação Internacional , Governo Estadual
20.
Ambio ; 41 Suppl 1: 33-45, 2012.
Artigo em Inglês | MEDLINE | ID: mdl-22314855

RESUMO

Stabilizing global greenhouse gas concentrations at levels to avoid significant climate risks will require massive "decarbonization" of all the major economies over the next few decades, in addition to the reduced emissions from other GHGs and carbon sequestration. Achieving the necessary scale of emissions reductions will require a multifaceted policy effort to support a broad array of technological and behavioral changes. Change on this scale will require sound, well-thought-out strategies. In this article, we outline some core principles, drawn from recent social science research, for guiding the design of clean technology policies, with a focus on energy. The market should be encouraged to make good choices: pricing carbon emissions and other environmental damage, removing distorting subsidies and barriers to competition, and supporting RD&D broadly. More specific policies are required to address particular market failures and barriers. For those technologies identified as being particularly desirable, some narrower RD&D policies are available.


Assuntos
Poluição do Ar/legislação & jurisprudência , Mudança Climática , Política Ambiental , Tecnologia , Poluição do Ar/economia , Aprendizagem , Marketing , Valores Sociais
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